Hybrid Hydrogel Electrolyte Based on Metal–Organic Supermolecular Self-Assembly and Polymer Chemical Cross-Linking for Rechargeable Aqueous Zn–MnO₂ Batteries

Multifunctional metal–organic supramolecular hydrogels have achieved great progress nowadays. However, their applications in aqueous batteries for flexible energy storage devices remain limited due to their unsatisfactory mechanical properties. Here, we report a rapid formation of supramolecular hydrogel by adenosine 5′-monophosphate (AMP) and manganese ions (Mn2+). Additionally, the AMP–Mn hydrogel is combined with chemical cross-linking poly(vinyl alcohol) (PVA) polymer networks to form an AMP–Mn/PVA hybrid hydrogel, which effectively solves the problems with regard to the mechanical properties and stability of metal–organic supramolecular hydrogels as well as self-healing of tough chemical cross-linking polymer networks. The AMP–Mn/PVA hybrid hydrogel served as the hydrogel electrolyte to fabricate flexible Zn–MnO2 batteries, which exhibit fast ion conductivity, excellent electrochemical stability, and robust mechanical strength, indicating feasible practical application prospects. This investigation provides a promising opportunity for the application of metal–organic supramolecular hydrogels in the field of energy storage.